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At least 451 records · Page 25Linked to original sources

Predictive analysis using chemical-gene interaction networks consistent with observed endocrine activity and mutagenicity of U.S. streams

In a recent U.S. Geological Survey/U.S. Environmental Protection Agency study assessing >700 organic compounds in 38 streams, in vitro assays indicated generally low estrogen, androgen, and glucocorticoid receptor activities, but identified 13 surface waters with 17β estradiol equivalent (E2Eq) activities greater than the 1 ng/L level of concern for feminization of male fish. Among the 36 samples assayed for mutagenicity in the Salmonella bioassay (reported here), 25% were considered mutagenic (statistically significant slope and at least a two-fold increase in revertants/plate). Endocrine and mutagenic activities of the water samples were well correlated with each other and with the total number and cumulative concentrations of detected chemical contaminants. To test the predictive utility of knowledgebase-leveraging approaches, site-specific predicted chemical-gene (pCGA) and predicted analogous pathway-linked (pPLA) association networks identified in the Comparative Toxicogenomics Database were compared with observed endocrine/mutagenic bioactivities. We evaluated pCGA/pPLA patterns among sites by cluster analysis and principal component analysis and grouped the pPLA into broad mode-of-action classes. Measured E2Eq and mutagenic activities correlated well with predicted pathways. The pPLA analysis also revealed correlations with signaling, metabolic, and regulatory groups, suggesting that other effects pathways may be associated with chemical contaminants in these waters and indicating the need for broader bioassay coverage to assess potential adverse impacts.

Environmental Science & Technology

Chemical and physical controls on mercury source signatures in stream fish from the northeastern United States

Streams in the northeastern U.S. receive mercury (Hg) in varying proportions from atmospheric deposition and legacy point sources, making it difficult to attribute shifts in fish concentrations directly back to changes in Hg source management. Mercury stable isotope tracers were utilized to relate sources of Hg to co-located fish and bed sediments from 23 streams across a forested to urban-industrial land-use gradient within this region. Mass-dependent isotopes (δ202Hg) in prey and game fish at forested sites were depleted (medians -0.95 and -0.83 ‰, respectively) in comparison to fish from urban-industrial settings (medians -0.26 and -0.38 ‰, respectively); the forested site group also had higher prey fish Hg concentrations. The separation of Hg isotope signatures in fish was strongly related to in-stream and watershed land-use indicator variables. Fish isotopes were strongly correlated with bed sediment isotopes, but the comparison of isotopic composition between fish and sediment was variable due to differing ecosystem-specific drivers controlling the extent of MeHg formation. The multivariable approach of analyzing watershed characteristics and stream chemistry reveals that the Hg isotope composition in fish is linked to current and historic Hg sources in the northeastern U.S. and can be used to trace bioaccumulated Hg.

Environmental Science & Technology

Wintering in the western subarctic pacific increases mercury contamination of Red-legged Kittiwakes

Marine methylmercury concentrations vary geographically and with depth, exposing organisms to different mercury levels in unique habitats. Red-legged kittiwakes (Rissa brevirostris), a specialist predator, forage on fish and invertebrates from the mesopelagic zone, a part of the ocean with elevated methylmercury concentrations. We used kittiwakes as bioindicators of MeHg concentrations in remote mesopelagic systems by examining how wintering distribution and habitat affected kittiwakes’ mercury exposure. In 2011-2017, we sampled winter-grown feathers on St. George Island, Alaska, from birds equipped with geolocation loggers. We measured total mercury (THg) and nitrogen stable in nape and head feathers grown during winter, respectively. THg concentration of kittiwake nape feathers averaged 4.61 ± 0.97 µg/g dry weight. Hierarchical cluster analysis was used to classify winter habitats with remotely sensed environmental variables along each bird’s track. Five habitat clusters were identified. Birds that spent more time in the Western Subarctic Gyre and those that wintered further south had elevated THg concentrations. In contrast to THg, trophic level varied annually but did not show strong spatial patterns. Our results documented spatial variability in THg exposure based on the oceanic wintering locations of red-legged kittiwakes and highlight their use as a bioindicator of MeHg across ocean basins.

Alaska

Using age tracers and decadal sampling to discern trends in nitrate, arsenic and uranium in groundwater beneath irrigated cropland

Repeat sampling and age tracers were used to examine trends in nitrate, arsenic and uranium concentrations in groundwater beneath irrigated cropland. Much higher nitrate concentrations in shallow modern groundwater were observed at both the Columbia Plateau and High Plains sites (median values of 10.2 and 15.4 mg/L as N, respectively) than in groundwater that recharged prior to the onset of intensive irrigation (median values of <1 and <4 mg/L as N, respectively). Repeat sampling of these well networks indicates that high nitrate concentrations in modern, shallow groundwater have been sustained for decades, posing a future risk to older, deeper groundwater used for drinking water. In fact, nitrate concentrations in older modern water (30-60 years since recharge) at the High Plains site have increased in the last decade. Groundwater irrigated areas in the Columbia Plateau tend to have higher nitrate concentrations than surface-water irrigated areas suggesting that repeated dissolution of land applied fertilizer during recirculation may be an important factor causing high nitrate concentrations in groundwater. Mobilization of uranium and arsenic by land surface activities is suggested by the higher concentrations of these constituents in modern, shallow groundwater than in older, deeper groundwater at the Columbia Plateau site. Bicarbonate concentrations in modern groundwater are positively correlated with uranium (r=0.72, p<0.01), suggesting bicarbonate may mobilize uranium in this system. A positive correlation between arsenic and phosphorus concentrations in modern groundwater (r=0.55, p<0.01) suggests that phosphate from fertilizer outcompetes arsenate for sorption sites, mobilizing sorbed arsenic derived from past pesticide use or other sources.

Environmental Science and Technology

Vertical distribution of microplastics in the water column and surficial sediment from the Milwaukee River basin to Lake Michigan

Microplastic contamination was studied along a freshwater continuum from inland streams to the Milwaukee River estuary to Lake Michigan, and vertically from the water surface, water subsurface and sediment. Microplastics were detected in all 96 water samples and nine sediment samples collected. Results indicated a gradient of polymer presence with depth: low-density particles decreased from water surface to subsurface to sediment, and high-density particles had the opposite result. Polymer identification results indicated water surface and subsurface samples were dominated by low-density polypropylene particles and sediment samples were dominated by more dense polyethylene terephthalate particles. Of the five particle-type categories (fragments, films, foams, pellets/beads and fibers/lines), fibers/lines were the most common particle type and were present in every water and sediment sample collected. Fibers represented 45% of all particles in water samples and were distributed vertically throughout the water column regardless of density. Sediment samples were dominated by black foams (66%, identified as styrene-butadiene rubber, SBR) and to a lesser extent fibers/lines (29%) with approximately 89% of all the sediment particles coming from polymers with densities greater than 1.1 g cm-3. Results demonstrated polymer density influenced partitioning between water surface and subsurface and the underlying surficial sediment and the common practice of sampling only the water surface can result in substantial bias, especially in estuarine, harbor and lake locations where water surface concentrations tend to overestimate mean water column concentrations.

Wisconsin

History and sources of co-occurring pesticides in an abstraction well unravelled by age distributions of depth specific groundwater samples

When groundwater-based drinking water supply becomes contaminated, the timing and source of contamination are obvious questions. However, contaminants often have diffuse sources and different contaminants may have different sources even in a single groundwater well, making these questions complicated to answer. Age dating of groundwater has been used to reconstruct contaminant travel times to wells; however, critics have highlighted that groundwater flow is often complex with mixing of groundwater of different ages. In drinking water wells, where water is typically abstracted from a large depth interval, such mixing is even more problematic. We present a way to overcome some of the obstacles in identifying the source and age of contaminants in drinking water wells by combining depth-specific sampling with age tracer modeling, particle tracking simulations, geological characterization, and contaminant properties. This multitool approach was applied to a drinking water well, where bentazon and dichlorprop contamination was found to have different pollutant sources and release histories, even though both pesticides can be associated with the same land use. Bentazon was derived from recent application to a golf course, while dichlorprop was derived from agricultural use more than 30 years ago. The advantages, limitations, and pitfalls of the proposed course of action are then further discussed.

Environmental Science & Technology

High-frequency data reveal deicing salts drive elevated specific conductance and chloride along with pervasive and frequent exceedances of the U.S. Environmental Protection Agency aquatic life criteria for chloride in urban streams

Increasing specific conductance (SC) and chloride concentrations [Cl] negatively affect many stream ecosystems. We characterized spatial variability in SC, [Cl], and exceedances of Environmental Protection Agency [Cl] criteria using nearly 30 million high-frequency observations (2–15 min intervals) for SC and modeled [Cl] from 93 sites across three regions in the eastern United States: Southeast, Mid-Atlantic, and New England. SC and [Cl] increase substantially from south to north and within regions with impervious surface cover (ISC). In the Southeast, [Cl] weakly correlates with ISC, no [Cl] exceedances occur, and [Cl] concentrations are constant with time. In the Mid-Atlantic and New England, [Cl] and [Cl] exceedances strongly correlate with ISC. [Cl] criteria are frequently exceeded at sites with greater than 9–10% ISC and median [Cl] higher than 30–80 mg/L. Tens to hundreds of [Cl] exceedances observed annually at most of these sites help explain previous research where stream ecosystems showed changes at (primarily nonwinter) [Cl] as low as 30–40 mg/L. Mid-Atlantic chronic [Cl] exceedances occur primarily in December–March. In New England, exceedances are common in nonwinter months. [Cl] is increasing at nearly all Mid-Atlantic and New England sites with the largest increases at sites with higher [Cl].

Environmental Science and Technology

Trophodynamics of per- and polyfluoroalkyl substances in the food web of a large Atlantic slope river

Per- and polyfluoroalkyl substances (PFASs) have attracted scientific and regulatory attention due to their persistence, bioaccumulative potential, toxicity, and global distribution. We determined the accumulation and trophic transfer of 14 PFASs (5 short-chain and 9 long-chain) within the food web of the Yadkin-Pee Dee River of North Carolina and South Carolina, US. Food web components and pathways were determined by stable isotope analyses of producers, consumers, and organic matter. Analyses of water, sediment, organic matter, and aquatic biota revealed that PFASs were prevalent in all food web compartments. Biofilm, an aggregation of bacteria, fungi, algae, and protozoans and a basal resource for the aquatic food web, showed high PFAS accumulation (in 10 of 14 compounds), particularly for perfluorooctanoic acid, with the greatest mean concentration of 463.73 ng/g. The food web compartment with the most detections and greatest concentrations of PFASs was aquatic insects; all 14 PFASs were detected in individual aquatic insect samples (range of <limit of detection [<LOD] to 1670.10 ng/g of wet weight [WW]). These findings may suggest a trophic link between biofilm PFASs and aquatic insect PFASs. Individual fish tissue samples ranged from <LOD to 797.00 ng/g of WW, where perfluorooctanesulfonate (PFOS) was the dominant PFAS among all samples (64%). The ova of an imperiled fish, the robust redhorse ( Moxostoma robustum ), had concentrations of 10 PFASs (range of <LOD to 482.88 ng/g of WW) and the highest PFOS concentration (482.88 ng/g of WW), indicating a likely maternal transfer. The trophic magnification factors (TMFs) calculated in this study showed that various taxa accumulated PFAS compounds differently. PFBS, a short-chain PFAS compound that would presumably exhibit lesser TMFs, had nine values among our compartments and organisms >1.0 (range of 0.57 to 2.33); it is possible that an unmeasured PFBS precursor may be accumulating in biota and metabolizing to PFBS, leading to a higher than expected TMFs for this compound. Our findings demonstrate the prevalence of PFASs in a freshwater food web with potential implications for ecological and human health.

North Carolina, South Carolina

Molecular identification of water-extractable organic carbon from thermally heated soils: C-13 NMR and accurate mass analyses find benzene and pyridine carboxylic acids

To simulate the effects of wildfire on the combustion process in soils and their potential to leach organic compounds into streams and groundwater, mineral soil samples were heated at temperatures of 150–550 °C. Then, the soils were leached with deionized water, filtered, and analyzed for dissolved organic carbon. The water extract was concentrated by both XAD-8 and XAD-4 resins and analyzed by C-13 nuclear magnetic resonance and liquid chromatography time-of-flight mass spectrometry. Approximately 15–20% of the water-extractable organic carbon was identified as benzene dicarboxylic acids, tricarboxylic acids, and tetracarboxylic acid isomers, commonly called BPCAs. Also identified were isomers of pyridine dicarboxylic acids and tricarboxylic acids (PCAs). The conversion of soil organic carbon to BPCAs occurs at 250 °C and reaches a maximum between 350 and 450 °C. At higher temperatures (>450 °C), the BPCA concentrations decrease, suggesting decarboxylation and conversion to carbon dioxide and water. This is the first report of BPCAs and PCAs in water-extractable organic carbon from thermally altered soil and suggest that these compounds are possible candidates for further water-quality studies in watersheds affected by wildfire. Finally, BPCAs and PCAs could contribute to the black carbon and nitrogen in seawater and are worthy of future investigation.

Environmental Science and Technology

Landscape drivers of dynamic change in water quality of US rivers

Water security is a top concern for social well-being and dramatic changes in the availability of freshwater have occurred as a result of human uses and landscape management. Elevated nutrient loading and perturbations to major ion composition have resulted from human activities and have degraded freshwater resources. This study addresses the emerging nature of stream water quality in the 21st century through analysis of concentrations and trends in a wide variety of constituents in streams and rivers of the U.S. Concentrations of fifteen separate water quality parameters including nutrients, major ions, sediment, and specific conductance were analyzed over the period 1982-2012 and a targeted trend analysis was performed from 1992-2012. Although environmental policy is geared toward addressing the long-standing problem of nutrient overenrichment, these efforts have had uneven success, with decreasing nutrient concentrations at urbanized sites and little to no change at agricultural sites. However, freshwaters are being salinized rapidly in all human-dominated land use types. Increasing salinity negatively affects biodiversity, mobilizes sediment-bound contaminants, and increases lead contamination of drinking water but the effects are poorly quantified. Therefore, while efforts to control nutrients are ongoing, rapid salinity increases are ushering in a new set of poorly-defined issues.

Environmental Science & Technology

Septic systems and rainfall influence human fecal markers and indicator organisms occurrence in private wells in southeastern Pennsylvania

In the United States approximately 48 million people are served by private wells. Unlike public water systems, private well water quality is not monitored and there are few studies on the extent and sources of contamination of private wells. We extensively investigated five private wells to understand the variability in microbial contamination, the role of septic systems as sources of contamination, and the effect of rainfall on well water quality. From 2016-2017, weekly or biweekly samples (n= 105) were collected from 5 private wells in rural Pennsylvania. Samples were tested for general water quality parameters, conventional and sewage-associated microbial indicators, and human pathogens. Total coliforms, human Bacteroides (HF183), and pepper mild mottle virus were detected at least once in all wells. Regression revealed significant relationships between HF183 and rainfall 8-14 days prior to sampling and between total coliforms and rainfall 8-14 or 0-14 days prior to sampling. Dye tracer studies at 3 wells confirmed the impact of household septic systems on well contamination. Microbiological measurements, chemical water quality data, and dye tracer tests provide evidence of human fecal contamination in the private wells studied, suggesting that household septic systems are the source of this contamination.

Pennsylvania

Assessing the impact of drought on arsenic exposure from private domestic wells in the conterminous United States

This study assesses the potential impact of drought on arsenic exposure from private domestic wells by using a previously developed statistical model that predicts the probability of elevated arsenic concentrations (>10 μg per liter) in water from domestic wells located in the conterminous United States (CONUS). The application of the model to simulate drought conditions used systematically reduced precipitation and recharge values. The drought conditions resulted in higher probabilities of elevated arsenic throughout most of the CONUS. While the increase in the probability of elevated arsenic was generally less than 10% at any one location, when considered over the entire CONUS, the increase has considerable public health implications. The population exposed to elevated arsenic from domestic wells was estimated to increase from approximately 2.7 million to 4.1 million people during drought. The model was also run using total annual precipitation and groundwater recharge values from the year 2012 when drought existed over a large extent of the CONUS. This simulation provided a method for comparing the duration of drought to changes in the predicted probability of high arsenic in domestic wells. These results suggest that the probability of exposure to arsenic concentrations greater than 10 μg per liter increases with increasing duration of drought. These findings indicate that drought has a potentially adverse impact on the arsenic hazard from domestic wells throughout the CONUS.

Conterminous United States

Contaminant subsidies to riparian food webs in Appalachian streams impacted by mountaintop removal coal mining

Selenium is highly elevated in Appalachian streams and stream organisms that receive alkaline mine drainage from mountaintop removal coal mining compared to unimpacted streams in the region. Adult aquatic insects can be important vectors of waterborne contaminants to riparian food webs, yet pathways of Se transport and exposure of riparian organisms are poorly characterized. We investigated Se concentrations in stream and riparian organisms to determine whether mining extent increased Se uptake in stream biofilms and insects and if these insects were effective Se biovectors to riparian spiders. Biofilm Se concentration increased (p = 0.006) with mining extent, reaching a maximum value of 16.5 μg/g of dw. Insect and spider Se increased with biofilm Se (p = 0.004, p = 0.003), reaching 95 and 26 μg/g of dw, respectively, in mining-impacted streams. Adult insect biomass was not related to mining extent or Se concentrations in biofilm. Even though Se concentrations in aquatic insects were significantly and positively related to mining extent, aquatic insect Se flux was not associated with mining extent because the mass of emerging insects did not change appreciably over the mining gradient. Insect and spider Se concentrations were among the highest reported in the literature, regularly exceeding the bird Se dietary risk threshold of 5 μg/g of dw. Risks of Se exposure and toxicity related to mining are thus not constrained to aquatic systems but extend to terrestrial habitats and food webs.

Environmental Science & Technology

Synthesis of maternal transfer of mercury in birds: Implications for altered toxicity risk

Maternal transfer is the predominant route of methylmercury (MeHg) exposure to offspring. We reviewed and synthesized published and unpublished data on maternal transfer of MeHg in birds. Using paired samples of females’ blood (n=564) and their eggs (n=1814) from 26 bird species in 6 taxonomic orders, we conducted a meta-analysis to evaluate whether maternal transfer of MeHg to eggs differed among species and caused differential toxicity risk to embryos. Total mercury (THg) concentrations in eggs increased with maternal blood THg concentrations; however, the proportion of THg transferred from females to their eggs differed among bird taxa and with maternal THg exposure. Specifically, a smaller proportion of maternal THg was transferred to eggs with increasing female THg concentrations. Additionally, the proportion of THg that was transferred to eggs at the same maternal blood THg concentration differed among taxonomic orders, with waterfowl (Anseriformes) transferring up to 382% more THg into their eggs than songbirds (Passeriformes). We provide equations to predict THg concentrations in eggs using female blood THg concentrations, and vice versa, which may help translate toxicity benchmarks across tissues and life stages. Our results indicate that toxicity risk of MeHg can vary among bird taxa due to differences in the maternal transfer of MeHg to offspring.

Environmental Science & Technology

Lifetime chronicles of selenium exposure linked to deformities in an imperiled migratory fish

Aquatic ecosystems worldwide face growing threats from elevated levels of contaminants from human activities. Toxic levels of selenium (Se) shown to cause deformities in birds, fish, and mammals can transfer from parents to progeny during embryonic development or accumulate through Se-enriched diets. For migratory species that move across landscapes, tracking exposure to elevated Se is vital to mitigating vulnerabilities. Yet, traditional toxicological investigations resolve only recent Se exposure. Here, we use a novel combination of X-ray fluorescence microscopy and depositional chronology in a biomineral to reveal for the first time provenance, life stage, and duration of toxic Se exposure over the lifetime of an organism. Spinal deformities observed in wild Sacramento Splittail ( Pogonichthys macrolepidotus ), an imperiled migratory minnow, were attributed to elevated Se acquired through maternal transfer and juvenile feeding on contaminated prey. This novel approach paves the way for diagnosing sources, pathways, and potential for a cumulative exposure of Se relevant for conservation.

California

Seasonal dynamics and interannual variability in mercury concentrations and loads through a three-reservoir complex

The Hells Canyon Complex (HCC) along the Snake River (Idaho-Oregon border, USA) encompasses three successive reservoirs that seasonally stratify, creating anoxic conditions in the hypolimnion that promote methylmercury (MeHg) production. This study quantified seasonal dynamics and interannual variability in mercury concentrations (inorganic divalent mercury (IHg) and MeHg) and loads at four reservoir inflow and outflow locations through the HCC (2014-2017). We observed (1) that the HCC is a net sink for both IHg and MeHg, (2) interannual variability in IHg and MeHg loads largely reflecting streamflow conditions, and (3) seasonal variability in particulate IHg loading at the inflow (greatest from February to April) and MeHg export from the outflow (greatest from September to December) of the HCC. Seasonal export of MeHg was evidenced by increases in monthly mean concentrations of unfiltered MeHg (approximately twofold) and the percentage of total mercury (THg) as MeHg (≥ fourfold) coincident with reservoir destratification. Despite evidence of seasonal export of MeHg from the HCC, annual loads indicate a 42% decrease in unfiltered MeHg from HCC inflow to outflow. Results from this study improve the understanding of seasonal variability in mercury transport through and transformation within a reservoir complex.

Idaho, Oregon

Mercury export from Arctic great rivers

Land–ocean linkages are strong across the circumpolar north, where the Arctic Ocean accounts for 1% of the global ocean volume and receives more than 10% of the global river discharge. Yet estimates of Arctic riverine mercury (Hg) export constrained from direct Hg measurements remain sparse. Here, we report results from a coordinated, year-round sampling program that focused on the six major Arctic rivers to establish a contemporary (2012–2017) benchmark of riverine Hg export. We determine that the six major Arctic rivers exported an average of 20 000 kg y –1 of total Hg (THg, all forms of Hg). Upscaled to the pan-Arctic, we estimate THg flux of 37 000 kg y –1 . More than 90% of THg flux occurred during peak river discharge in spring and summer. Normalizing fluxes to watershed area (yield) reveals higher THg yields in regions where greater denudation likely enhances Hg mobilization. River discharge, suspended sediment, and dissolved organic carbon predicted THg concentration with moderate fidelity, while suspended sediment and water yields predicted THg yield with high fidelity. These findings establish a benchmark in the face of rapid Arctic warming and an intensifying hydrologic cycle, which will likely accelerate Hg cycling in tandem with changing inputs from thawing permafrost and industrial activity.

Environmental Science & Technology

Biofilms provide new insight into pesticide occurrence in streams and links to aquatic ecological communities

Streambed sediment is commonly analyzed to assess occurrence of hydrophobic pesticides and risks to aquatic communities. However, stream biofilms also have the potential to accumulate pesticides and may be consumed by aquatic organisms. To better characterize risks to aquatic life, the U.S. Geological Survey Regional Stream Quality Assessment measured 93 current-use and 3 legacy pesticides in bed sediment and biofilm from 54 small streams in California across a range of land-use settings. On average, 4 times as many current-use pesticides were detected in biofilm at a site (median of 2) as in sediment (median of 0.5). Of 31 current-use pesticides detected, 20 were detected more frequently in biofilm than sediment and 10 equally frequently. Pyrethroids as a class were the most potentially toxic to benthic invertebrates, and of the nine pyrethroids detected, seven occurred more frequently in biofilm than sediment. We constructive General Additive Models to investigate relations between pesticides and six metrics of benthic community structure. Pesticides in biofilm improved fit in four of the six models, and pesticides in sediment improved fit in two. The results indicate that sampling of stream biofilms can complement bed-sediment sampling by identifying more current-use pesticides present and better estimating ecological risks.

California